Influence of Phospholipid Composition on Self-Assembly and Energy-Transfer Efficiency in Networks of Light-Harvesting 2 Complexes

被引:30
作者
Sumino, Ayumi [1 ]
Dewa, Takehisa [1 ,2 ]
Noji, Tomoyasu [1 ]
Nakano, Yuki [1 ]
Watanabe, Natsuko [1 ]
Hildner, Richard [3 ,4 ]
Boesch, Nils [3 ,4 ]
Koehler, Juergen [3 ,4 ]
Nango, Mamoru [1 ]
机构
[1] Nagoya Inst Technol, Grad Sch Engn, Dept Frontier Mat, Showa Ku, Nagoya, Aichi 4668555, Japan
[2] Japan Sci & Technol Agcy, PRESTO, Kawaguchi, Saitama 3320012, Japan
[3] Univ Bayreuth, D-95440 Bayreuth, Germany
[4] Univ Bayreuth, BIMF, D-95440 Bayreuth, Germany
基金
日本科学技术振兴机构;
关键词
ELECTRONICALLY EXCITED-STATES; TIME-RESOLVED SPECTROSCOPY; LH2; COMPLEXES; MEMBRANE-PROTEIN; RHODOPSEUDOMONAS-PALUSTRIS; PHOTOSYNTHETIC APPARATUS; RHODOSPIRILLUM-RUBRUM; CRYSTAL-STRUCTURE; PURPLE BACTERIA; ACIDOPHILA;
D O I
10.1021/jp4047819
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In the photosynthetic membrane of purple bacteria networks of light-harvesting 2 (LH2) complexes capture the sunlight and transfer the excitation energy. In order to investigate the mutual relationship between the supramolecular organization of the pigment-protein complexes and their biological function, the LH2 complexes were reconstituted into three types of phospholipid membranes, consisting of L-alpha-phosphatidylglycerol (PG), L-alpha-phosphatidylcholine (PC), and L-alpha-phosphatidylethanolamine (PE)/PG/cardiolipin (CL). Atomic force microscopy (AFM) revealed that the type of phospholipids had a crucial influence on the clustering tendency of the LH2 complexes increased from PG over PC to PE/PG/CL, where the LH2 complexes formed large, densely packed clusters. Time-resolved spectroscopy uncovered a strong quenching of the LH2 fluorescence that is ascribed to singlet-singlet and singlet-triplet annihilation by an efficient energy transfer between the LH2 complexes in the artificial membrane systems. Quantitative analysis reveals that the intercomplex energy transfer efficiency varies strongly as a function of the morphology of the nanostructure, namely in the order PE/PG/CL > PC > PG, which is in line with the clustering tendency of LH2 observed by AFM. These results suggest a strong influence of the phospholipids on the self-assembly of LH2 complexes into networks and concomitantly on the intercomplex energy transfer efficiency.
引用
收藏
页码:10395 / 10404
页数:10
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